抗原变异可使得多种致病微生物易于逃避宿主免疫应答。表达在感染红细胞表面的恶性疟原虫红细胞表面蛋白1（PfPMP1）与感染红细胞、内皮细胞、树突状细胞以及胎盘的单个或多个受体作用，在黏附及免疫逃避中起关键的作用。每个单倍体基因组var基因家族编码约60种成员，通过启动转录不同的var基因变异体为抗原变异提供了分子基础。

疟原虫var基因转换速率变化导致抗原变异[英]／Paul H, Robert P, Christodoulou Z, et al//Proc Natl Acad Sci U S A

A revolution in novel nanoparticles and colloidal building blocks has been enabled by recent breakthroughs in particle synthesis These new particles are poised to become the ‘atoms’ and ‘molecules’ of tomorrow’s materials if they can be successfully assembled into useful structures Here, we discuss the recent progress made in the synthesis of nanocrystals and colloidal particles and draw analogies between these new particulate building blocks and better-studied molecules and supramolecular objects We argue for a conceptual framework for these new building blocks based on anisotropy attributes and discuss the prognosis for future progress in exploiting anisotropy for materials design and assembly

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Anisotropy of building blocks and their assembly into complex structures

Journal of Physics Condensed Matter: Preface

A challenging goal in materials chemistry and physics is spontaneously to form intended superstructures from designed building blocks. In fields such as crystal engineering and the design of porous materials, this typically involves building blocks of organic molecules, sometimes operating together with metallic ions or clusters. The translation of such ideas to nanoparticles and colloidal-sized building blocks would potentially open doors to new materials and new properties, but the pathways to achieve this goal are still undetermined. Here we show how colloidal spheres can be induced to self-assemble into a complex predetermined colloidal crystal-in this case a colloidal kagome lattice-through decoration of their surfaces with a simple pattern of hydrophobic domains. The building blocks are simple micrometre-sized spheres with interactions (electrostatic repulsion in the middle, hydrophobic attraction at the poles, which we call 'triblock Janus') that are also simple, but the self-assembly of the spheres into an open kagome structure contrasts with previously known close-packed periodic arrangements of spheres. This open network is of interest for several theoretical reasons. With a view to possible enhanced functionality, the resulting lattice structure possesses two families of pores, one that is hydrophobic on the rims of the pores and another that is hydrophilic. This strategy of 'convergent' self-assembly from easily fabricated colloidal building blocks encodes the target supracolloidal architecture, not in localized attractive spots but instead in large redundantly attractive regions, and can be extended to form other supracolloidal networks.

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Directed self-assembly of a colloidal kagome lattice

Controlling interparticle interactions, aggregation and cluster formation is of central importance in a number of areas, ranging from cluster formation in various disease processes to protein crystallography and the production of photonic crystals. Recent developments in the description of the interaction of colloidal particles with short-range attractive potentials have led to interesting findings including metastable liquid-liquid phase separation and the formation of dynamically arrested states (such as the existence of attractive and repulsive glasses, and transient gels). The emerging glass paradigm has been successfully applied to complex soft-matter systems, such as colloid-polymer systems and concentrated protein solutions. However, intriguing problems like the frequent occurrence of cluster phases remain. Here we report small-angle scattering and confocal microscopy investigations of two model systems: protein solutions and colloid-polymer mixtures. We demonstrate that in both systems, a combination of short-range attraction and long-range repulsion results in the formation of small equilibrium clusters. We discuss the relevance of this finding for nucleation processes during protein crystallization, protein or DNA self-assembly and the previously observed formation of cluster and gel phases in colloidal suspensions.

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Equilibrium cluster formation in concentrated protein solutions and colloids

Polycrystals of thin colloidal deposits, with thickness controlled by spin-coating speed, exhibit axial symmetry with local 4-fold and 6-fold symmetric structures, termed orientationally correlated polycrystals (OCPs). While spin-coating is a very facile technique for producing large-area colloidal deposits, the axial symmetry prevents us from achieving true long-range order. To obtain true long-range order, we break this axial symmetry by introducing a patterned surface topography and thus eliminate the OCP character. We then examine symmetry-independent methods to quantify order in these disordered colloidal deposits. We find that all the information in the bond-orientational order parameters is well captured by persistent homology analysis methods that only use the centers of the particles as input data. It is expected that these methods will prove useful in characterizing other disordered structures.

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Quantifying disorder in colloidal films spin-coated onto patterned substrates

Cluster Phases in Colloids and Proteins

The in-cell environment is crowded with macromolecules, and the consequent reduction in free volume, based on the hard-sphere paradigm, is central to understanding macromolecular motions. A much-used model crowder, Ficoll, often assumed to be a compact, if not rigid, colloidal particle, is studied by rheology, small-angle neutron scattering, nuclear magnetic resonance diffusometry, and relaxometry. We find that the Ficoll suspension viscosity scales linearly with concentration cF in the dilute limit and as ∼cF3.8 at high cF, i.e, consistent with the 15/4 (de Gennes) scaling for a reptating polymer. The form factor of Ficoll, obtained via small-angle neutron scattering (SANS), resembles either a Gaussian polymer or a soft polymer blob. From NMR diffusion measurements, we obtain an effective volume fraction for Ficoll that accounts for Ficoll-bound water in two ways and show that each results in a volume occupancy of 60% to 70% in the crowding limit, much larger than the traditionally reported values of around 30%. If we persist with the colloid paradigm and examine the dependence of the zero-q structure factor obtained via SANS in terms of this effective volume fraction, we find that only a combination of particle softness and interparticle attractions, quantified using a computational model, can replicate the experimental S(0). The stark difference between effective and traditional volume occupancies affects the interpretation of previous experiments on macromolecular crowding and might explain the intriguing non-monotonicity observed in the dependence of protein relaxation rates on crowder concentration. 

Is Ficoll a Colloid or Polymer? A Multitechnique Study of a Prototypical Excluded-Volume Macromolecular Crowder

In this work we generate stable and monodisperse water-in-oil emulsions using a co-flowing geometry that produced droplet sizes between 13 μm and 250 μm. The drops survived transfer to NMR tubes and were stable for at least 26 hours, enabling the performance of pulsed-field-gradient NMR experiments in addition to microscopy. The drops sizes achieved as a function of flow rate agree well with a simple model for droplet generation: this yields a precise measure of the interfacial tension. The design of a cell mimetic environment with nano-scale confinement has also been demonstrated with diffusion measurements on macromolecules (PEG and Ficoll70) within droplets that are further structured internally using agarose gel networks. Containing the agarose gel in droplets appears to provide very reproducible and homogeneous network environments, enabling quantitative agreement of Ficoll70 dynamics with a theoretical model, with no fit parameters, and, with PEG, yielding a systematic polymer-size dependent slowing down in the network. This is in contrast with bulk agarose, where identical macromolecular diffusion measurements indicate the presence of heterogeneities with water pockets.

Realization of a stable, monodisperse water-in-oil droplet system with micro-scale and nano-scale confinement for tandem microscopy and diffusion NMR studies

We present a new, extremely sensitive optical method to study the nematic-smectic-A (NA) phase transition in liquid crystals. In this new technique, we monitor nematic director fluctuations as a function of temperature as we approach the NA transition. We show that the NA transition in the liquid crystal 8CB (which has a small nematic range) is clearly first order, well within the resolution of the experiment. This is contrary to previous calorimetric measurements but confirms an earlier dynamical measurement. We characterize the strength of the phase transition by a dimensionless, technique-independent quantity t 0 = (T NA - T*)/T NA. For 8CB, we measure t 0 = (6 ± 2) × 10−6.

Anand Yethiraj

Papers

Quantifying disorder in colloidal films spin-coated onto patterned substrates

Cluster Phases in Colloids and Proteins

Is Ficoll a Colloid or Polymer? A Multitechnique Study of a Prototypical Excluded-Volume Macromolecular Crowder

Realization of a stable, monodisperse water-in-oil droplet system with micro-scale and nano-scale confinement for tandem microscopy and diffusion NMR studies

Using Nematic Director Fluctuations as a Sensitive Probe of the Nematic-Smectic-a Phase Transition in Liquid Crystals